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Natural Attenuation of 2,4-Dichlorophenol in Fe-Rich Soil during Redox Oscillations: Anoxic-Oxic Coupling Mechanism. 富铁土壤中 2,4-二氯苯酚在氧化还原振荡过程中的自然衰减:缺氧-缺氧耦合机制。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-19 DOI: 10.1021/acs.est.4c03244
Jingyi Zhang, Xiaoyun Xu, Jun Liang, Wenfeng Huang, Ling Zhao, Hao Qiu, Xinde Cao

Natural attenuation of organic contaminants can occur under anoxic or oxic conditions. However, the effect of the coupling anoxic-oxic process, which often happens in subsurface soil, on contaminant transformation remains poorly understood. Here, we investigated 2,4-dichlorophenol (2,4-DCP) transformation in Fe-rich soil under anoxic-oxic alternation. The anoxic and oxic periods in the alternating system showed faster 2,4-DCP transformation than the corresponding control single anoxic and oxic systems; therefore, a higher transformation rate (63.4%) was obtained in the alternating system relative to control systems (27.9-42.4%). Compared to stable pH in the alternating system, the control systems presented clear OH- accumulation, caused by more Fe(II) regeneration in the control anoxic system and longer oxygenation in the control oxic system. Since 2,4-DCP was transformed by ion exchangeable Fe(II) in soil via direct reduction in the anoxic process and induced ·OH oxidation in the oxic process, OH- accumulation was unbeneficial because it competed for proton with direct reduction and inhibited OH generation via complexing with Fe(II). However, the alternating system exhibited OH--buffering capacity via anoxic-oxic coupling processes because the subsequent oxic periods intercepted Fe(II) regeneration in anoxic periods, while shorter exposure to O2 in oxic periods avoided excessive OH- generation. These findings highlight the significant role of anoxic-oxic alternation in contaminant attenuation persistently.

有机污染物的自然衰减可在缺氧或缺氧条件下发生。然而,人们对地下土壤中经常发生的缺氧-缺氧耦合过程对污染物转化的影响仍然知之甚少。在此,我们研究了缺氧-缺氧交替条件下富铁质土壤中 2,4-二氯苯酚(2,4-DCP)的转化情况。与对照组的单一缺氧和缺氧系统相比,交替系统中的缺氧和缺氧期的 2,4-DCP 转化速度更快;因此,与对照组(27.9%-42.4%)相比,交替系统中的转化率更高(63.4%)。与交替系统中稳定的 pH 值相比,对照系统中出现了明显的 OH- 积累,这是由于对照缺氧系统中铁(II)再生更多,而对照缺氧系统中氧合时间更长。由于 2,4-DCP 在缺氧过程中通过直接还原作用被土壤中的离子交换铁(II)转化,并在缺氧过程中诱导-OH 氧化,因此 OH- 积累是无益的,因为它与直接还原作用竞争质子,并通过与铁(II)络合抑制了-OH 的生成。然而,交替系统通过缺氧-缺氧耦合过程表现出 OH 缓冲能力,因为随后的缺氧期拦截了缺氧期的铁(II)再生,而在缺氧期较短的暴露于 O2 的时间则避免了过量 OH 的生成。这些发现凸显了缺氧-缺氧交替在污染物持续衰减中的重要作用。
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引用次数: 0
Microplastics Biofragmentation and Degradation Kinetics in the Plastivore Insect Tenebrio molitor. 微塑料在塑生昆虫 Tenebrio molitor 中的生物破碎和降解动力学。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-19 DOI: 10.1021/acs.est.4c05113
Bo-Yu Peng, Wen-Xiong Wang

The insect Tenebrio molitor possesses an exceptional capacity for ultrafast plastic biodegradation within 1 day of gut retention, but the kinetics remains unknown. Herein, we investigated the biofragmentation and degradation kinetics of different microplastics (MPs), i.e., polyethylene (PE), poly(vinyl chloride) (PVC), and poly(lactic acid) (PLA), in T. molitor larvae. The intestinal reactions contributing to the in vivo MPs biodegradation were concurrently examined by utilizing aggregated-induced emission (AIE) probes. Our findings revealed that the intestinal biofragmentation rates essentially followed the order of PLA > PE > PVC. Notably, all MPs displayed retention effects in the intestine, with PVC requiring the longest duration for complete removal/digestion. The dynamic rate constant of degradable MPs (0.2108 h-1 for PLA) was significantly higher than that of persistent MPs (0.0675 and 0.0501 h-1 for PE and PVC, respectively) during the digestive gut retention. Surprisingly,T. molitor larvae instinctively modulated their internal digestive environment in response to in vivo biodegradation of various MP polymers. Esterase activity and intestinal acidification both significantly increased following MPs ingestion. The highest esterase and acidification levels were observed in the PLA-fed and PVC-fed larvae, respectively. High digestive esterase activity and relatively low acidification levels inT. molitor larvae may, to some extent, contribute to more efficient MPs removal within the plastic-degrading insect. This work provided important understanding of MPs biofragmentation and intestinal responses to in vivo MPs biodegradation in plastic-degrading insects.

昆虫Tenebrio molitor在肠道滞留1天内具有超快的塑料生物降解能力,但其动力学仍然未知。在此,我们研究了不同微塑料(MPs),即聚乙烯(PE)、聚氯乙烯(PVC)和聚乳酸(PLA)在褐蝶幼虫体内的生物破碎和降解动力学。利用聚集诱导发射(AIE)探针同时检测了促进体内 MPs 生物降解的肠道反应。我们的研究结果表明,肠道生物破碎率基本上遵循聚乳酸 > 聚乙烯 > 聚氯乙烯的顺序。值得注意的是,所有主要成分在肠道中都有滞留效应,其中 PVC 需要最长的时间才能完全去除/消化。在消化肠道滞留期间,可降解多孔材料的动态速率常数(聚乳酸为 0.2108 h-1)明显高于持久性多孔材料(聚乙烯和聚氯乙烯分别为 0.0675 和 0.0501 h-1)。令人惊奇的是,褐飞虱幼虫在体内生物降解各种多孔质聚合物时,会本能地调节其内部消化环境。摄入多孔质聚合物后,酯酶活性和肠道酸化程度都明显增加。喂食聚乳酸和聚氯乙烯的幼虫的酯酶和酸化水平分别最高。在某种程度上,褐飞虱幼虫的高消化酯酶活性和相对较低的酸化水平可能有助于塑料降解昆虫更有效地清除MPs。这项研究为了解降解塑料昆虫体内MPs的生物破碎和肠道对MPs生物降解的反应提供了重要信息。
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引用次数: 0
Introducing ARTiMiS: A Low-Cost Flow Imaging Microscope for Microalgal Monitoring. 介绍 ARTiMiS:用于微藻监测的低成本流动成像显微镜。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-19 DOI: 10.1021/acs.est.4c01928
Benjamin Gincley, Farhan Khan, Elaine Hartnett, Autumn Fisher, Ameet J Pinto

Manual microscopy is the gold standard for phytoplankton monitoring in diverse engineered and natural environments. However, it is both labor-intensive and requires specialized training for accuracy and consistency, and therefore difficult to implement on a routine basis without significant time investment. Automation can reduce this burden by simplifying the measurement to a single indicator (e.g., chlorophyll fluorescence) measurable by a probe, or by processing samples on an automated cytometer for more granular information. The cost of commercially available flow imaging cytometers, however, poses a steep financial barrier to adoption. To overcome these labor and cost barriers, we developed ARTiMiS: the Autonomous Real-Time Microbial 'Scope. The ARTiMiS is a low-cost flow imaging microscopy-based platform with onboard software capable of providing taxonomically resolved quantitation of phytoplankton communities in real-time. ARTiMiS leverages novel multimodal imaging and onboard machine learning-based data processing that is currently optimized for a curated and expandable database of industrially relevant microalgae. We demonstrate its operational limits, performance in identification of laboratory-cultivated microalgae, and potential for continuous monitoring of complex microalgal communities in full-scale industrial cultivation systems.

人工显微镜是在各种工程和自然环境中监测浮游植物的黄金标准。然而,人工显微镜既耗费大量人力,又需要经过专门培训才能保证准确性和一致性,因此,如果不投入大量时间,就很难在日常工作中实施。自动化可将测量简化为探针可测量的单一指标(如叶绿素荧光),或在自动细胞仪上处理样本以获得更精细的信息,从而减轻这种负担。然而,市场上销售的流式成像细胞仪成本高昂,对采用该技术构成了巨大的经济障碍。为了克服这些人力和成本障碍,我们开发了 ARTiMiS:自主实时微生物 "范围"。ARTiMiS 是一种基于流式成像显微镜的低成本平台,带有板载软件,能够实时对浮游植物群落进行分类定量。ARTiMiS 利用新颖的多模态成像技术和基于板载机器学习的数据处理技术,目前已针对具有工业相关性的微藻数据库进行了优化和扩展。我们展示了它的操作限制、实验室培养微藻的识别性能,以及在大规模工业培养系统中持续监测复杂微藻群落的潜力。
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引用次数: 0
Long-term Application of Agricultural Amendments Regulate Hydroxyl Radicals Production during Oxygenation of Paddy Soils. 长期施用农业改良剂可调节水稻田土壤增氧过程中羟基自由基的产生。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-18 DOI: 10.1021/acs.est.4c03917
Ning Chen, Danyu Huang, Yu Zeng, Juan Wang, Guangxia Liu, Xiantang Liu, Tongliang Wu, Yan Gao, Guodong Fang, Yujun Wang, Dongmei Zhou

Hydroxyl radicals (OH) play a significant role in contaminant transformation and element cycling during redox fluctuations in paddy soil. However, these important processes might be affected by widely used agricultural amendments, such as urea, pig manure, and biochar, which have rarely been explored, especially regarding their impact on soil aggregates and associated biogeochemical processes. Herein, based on five years of fertilization experiments in the field, we found that agricultural amendments, especially coapplication of fertilizers and biochar, significantly increased soil organic carbon contents and the abundances of iron (Fe)-reducing bacteria. They also substantially altered the fraction of soil aggregates, which consequently enhanced the electron-donating capacity and the formation of active Fe(II) species (i.e., 0.5 M HCl-Fe(II)) in soil aggregates (0-2 mm), especially in small aggregates (0-3 μm). The highest contents of active Fe(II) species in small aggregates were mainly responsible for the highest OH production (increased by 1.7-2.4-fold) and naphthalene attenuation in paddy soil with coapplication of fertilizers and biochar. Overall, this study offers new insights into the effects of agricultural amendments on regulating OH formation in paddy soil and proposes feasible strategies for soil remediation in agricultural fields, especially in soils with frequent occurrences of redox fluctuations.

羟基自由基(-OH)在水稻土壤氧化还原波动过程中的污染物转化和元素循环中发挥着重要作用。然而,这些重要的过程可能会受到尿素、猪粪和生物炭等广泛使用的农业改良剂的影响,而这些改良剂对土壤团聚体和相关生物地球化学过程的影响却鲜有研究。在此,基于五年的田间施肥实验,我们发现农业改良剂,尤其是肥料和生物炭的共同施用,显著增加了土壤有机碳含量和铁(Fe)还原菌的丰度。它们还极大地改变了土壤团聚体的比例,从而增强了土壤团聚体(0-2 毫米),尤其是小团聚体(0-3 微米)的电子供能能力和活性铁(II)物种(即 0.5 M HCl-铁(II))的形成。在施用化肥和生物炭的水稻土中,小团聚体中活性铁(II)物种的含量最高,这主要是导致-OH 产生量最高(增加了 1.7-2.4 倍)和萘衰减量最高的原因。总之,本研究为农业改良剂调节水稻田土壤中 -OH 形成的效果提供了新的见解,并为农田土壤修复,尤其是经常发生氧化还原波动的土壤修复提出了可行的策略。
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引用次数: 0
Fingerprinting Organofluorine Molecules via Position-Specific Isotope Analysis. 通过位置特异性同位素分析对有机氟分子进行指纹识别。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-18 DOI: 10.1021/acs.est.4c02250
Cornelia Rasmussen, David Hoffman

Organofluorine substances are found in a wide range of materials and solvents commonly used in industry and homes, as well as pharmaceuticals and pesticides. In the environment, organofluorine molecules are now recognized as an important class of anthropogenic pollutants. Fingerprinting organofluorine compounds via their carbon isotope ratios (13C/12C) is crucial for correlating molecules with their source. Here we apply a 19F nuclear magnetic resonance spectroscopy (NMR) technique to obtain the first position-specific carbon isotope ratios for a diverse set of organofluorine molecules. In contrast to traditional isotope ratio mass spectrometry, the 19F NMR method provides 13C/12C isotope ratios at each carbon position where a C-F bond is present, and does not require fragmentation or combustion to CO2, overcoming challenges posed by the robust C-F covalent bonds. The method was validated with 2,2,2-trifluoroethanol, and applied to analyze heptafluorobutanoic acid, 5-fluorouracil and fipronil. Results reveal distinct intramolecular carbon isotope distributions, enabling differentiation of chemically identical molecules. Notably, the NMR method accurately analyzes carbon isotopes within target molecules despite impurities. Potential applications include the detection of counterfeit products and drugs, and ultimately pollution tracking in the environment.

有机氟物质广泛存在于工业和家庭常用的材料和溶剂以及药品和杀虫剂中。在环境中,有机氟分子现已被视为一类重要的人为污染物。通过碳同位素比(13C/12C)对有机氟化合物进行指纹识别,对于将分子与其来源联系起来至关重要。在这里,我们应用 19F 核磁共振光谱(NMR)技术首次获得了一组不同有机氟分子的特定位置碳同位素比值。与传统的同位素比质谱法不同,19F NMR 方法提供了存在 C-F 键的每个碳位置的 13C/12C 同位素比,而且不需要破碎或燃烧成 CO2,克服了坚固的 C-F 共价键带来的挑战。该方法用 2,2,2-三氟乙醇进行了验证,并应用于分析七氟丁酸、5-氟尿嘧啶和氟虫腈。结果显示,分子内的碳同位素分布各不相同,因此可以区分化学性质相同的分子。值得注意的是,尽管存在杂质,核磁共振方法仍能准确分析目标分子内的碳同位素。其潜在应用包括检测假冒产品和药物,以及最终追踪环境污染。
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引用次数: 0
Mixing due to Solution Switch Limits the Performance of Electrosorption for Desalination. 溶液切换导致的混合限制了电吸附脱盐的性能。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-18 DOI: 10.1021/acs.est.4c02681
Weifan Liu, Longqian Xu, Zezhou Yang, Xudong Zhang, Shihong Lin

Electrosorption (ES) is a research frontier in electrochemical separation, with proven potential applications in desalination, wastewater treatment, and selective resource extraction. However, due to the limited adsorption capacity of film electrodes, ES requires short circuiting or circuit reversal, accompanied by a solution switch between the feed solution and receiving solution, to sustain desalination over many charge-discharge cycles. In previously reported studies, solution switches have been commonly ignored to simplify experimental procedures, and their impacts on separation performance are thus not well understood. This study aims to provide a quantitative analysis of the impacts of mixing due to a solution switch on the performance of ES-based desalination. A numerical model of ES has been employed to evaluate the adverse effects of the solution switch on the desalination performance in three commonly used operation modes. The analysis reveals that the impacts of mixing due to solution-switch are more severe with a larger concentration difference between the desalinated water and the brine and provides insights into the effectiveness of increasing electrode loading or specific capacity in mitigating the detrimental impacts of mixing. Even with state-of-the-art systems, producing freshwater from seawater or even brackish water with medium-to-high salinity is practically challenging due to the presence of solution switch.

电吸附(ES)是电化学分离领域的一个研究前沿,在海水淡化、废水处理和选择性资源提取方面具有公认的应用潜力。然而,由于薄膜电极的吸附能力有限,电吸附需要短路或电路反转,并伴随着进料溶液和接收溶液之间的溶液切换,才能在多次充放电循环中维持海水淡化。在之前报道的研究中,为了简化实验程序,通常会忽略溶液开关,因此对其对分离性能的影响还不甚了解。本研究旨在定量分析溶液开关导致的混合对基于 ES 的海水淡化性能的影响。采用 ES 的数值模型来评估三种常用操作模式下溶液切换对海水淡化性能的不利影响。分析结果表明,当脱盐水和盐水之间的浓度差越大时,溶液切换导致的混合影响就越严重,并深入探讨了增加电极负载或比容量在减轻混合不利影响方面的有效性。由于溶液切换的存在,即使采用最先进的系统,从海水甚至中高盐度的苦咸水中生产淡水实际上也是一项挑战。
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引用次数: 0
Enhanced Aging of Black Carbon under Recent Clean Air Actions and Future Carbon Neutrality Scenario in China. 中国近期清洁空气行动和未来碳中和情景下黑碳的强化老化。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-18 DOI: 10.1021/acs.est.4c02030
Wenxiang Shen, Minghuai Wang, Xinyi Dong

China has implemented strict emission control measures, but it is unclear how they affect black carbon (BC) aging and light absorption. Here, we use the Community Atmosphere Model version 6 (CAM6) with the four-mode version of the Modal Aerosol Module coupled with machine learning (MAM4-ML) to simulate BC aging during 2011-2018 and 2050/2100 following a carbon neutrality scenario (SSP1-2.6), respectively. During 2011-2018, the mass ratio of coatings to BC (RBC) widely increased (5.4% yr-1) over the east of China. The increased secondary organic aerosol (SOA) coatings dominate (88%) the increased RBC, while the sulfate coatings decrease. The drivers of BC coating changes come from the different magnitudes of emission reductions in secondary aerosol precursors (i.e., volatile organic compounds (VOCs) and SO2) and BC. During 2011-2018, the increased RBC enhances the BC mass absorption cross section (MAC, 0.7% yr-1). In 2050/2100 for SSP1-2.6, emission control leads to further increased RBC (95/145%) and BC MAC (12/17%). For both 2011-2018 and 2050/2100, the enhanced BC MAC partly offsets the declining direct radiative effect (DRE) of BC due to direct emission reduction. As a result, the full impact of direct emission reductions of BC on BC DRE is only 75% for 2011-2018 and 90/94% for 2050/2100.

中国实施了严格的排放控制措施,但这些措施如何影响黑碳(BC)的老化和光吸收尚不清楚。在此,我们利用共同体大气模式第6版(CAM6)和结合机器学习的模态气溶胶模块四模式版本(MAM4-ML),分别模拟了2011-2018年和2050/2100年碳中和情景(SSP1-2.6)下的黑碳老化。在 2011-2018 年期间,中国东部地区涂层与 BC(RBC)的质量比广泛增加(5.4% yr-1)。二次有机气溶胶(SOA)涂层的增加主导了 RBC 的增加(88%),而硫酸盐涂层则有所减少。BC涂层变化的驱动因素来自于二次气溶胶前体(即挥发性有机化合物和二氧化硫)和BC的不同减排量。在 2011-2018 年期间,增加的 RBC 会提高 BC 质量吸收截面(MAC,0.7% yr-1)。在 2050/2100 年,对于 SSP1-2.6,排放控制会进一步增加 RBC(95/145%)和 BC MAC(12/17%)。在 2011-2018 年和 2050/2100 年,BC MAC 的增加部分抵消了直接减排导致 BC 直接辐射效应(DRE)的下降。因此,2011-2018 年和 2050/2100 年,直接减排对 BC 直接辐射效应的全部影响仅为 75%和 90/94%。
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引用次数: 0
Cadmium Isotope Fractionation during Adsorption onto Edge Sites and Vacancies in Phyllomanganate. 植物锰酸钾边缘位和空位吸附过程中的镉同位素分馏。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-18 DOI: 10.1021/acs.est.4c03808
Hui Yin, Xinran Yan, Chuanwei Zhu, Kideok D Kwon, Xueyuan Gu, Wei Zhao, Bruno Lanson, Wei Li, Jingyuan Ma, Yan Li, Jiangshan Li, Guohong Qiu, Xionghan Feng, Wenfeng Tan, Hanjie Wen, Qiaoyun Huang, Fan Liu

Cadmium (Cd) geochemical behavior is strongly influenced by its adsorption onto natural phyllomanganates, which contain both layer edge sites and vacancies; however, Cd isotope fractionation mechanisms at these sites have not yet been addressed. In the present work, Cd isotope fractionation during adsorption onto hexagonal (containing both types of sites) and triclinic birnessite (almost only edge sites) was investigated using a combination of batch adsorption experiments, extended X-ray absorption fine structure (EXAFS) spectroscopy, surface complexation modeling, and density functional theory (DFT) calculations. Light Cd isotopes are preferentially enriched on solid surfaces, and the isotope fractionation induced by Cd2+ adsorption on edge sites (Δ114/110Cdedge-solution = -1.54 ± 0.11‰) is smaller than that on vacancies (Δ114/110Cdvacancy-solution = -0.71 ± 0.21‰), independent of surface coverage or pH. Both Cd K-edge EXAFS and DFT results indicate the formation of double corner-sharing complexes on layer edge sites and mainly triple cornering-sharing complexes on vacancies. The distortion of both complexes results in the negative isotope fractionation onto the solids, and the slightly longer first Cd-O distances and a smaller number of nearest Mn atoms around Cd at edge sites probably account for the larger fractionation magnitude compared to that of vacancies. These results provide deep insights into Cd isotope fractionation mechanisms during interactions with phyllomanganates.

镉(Cd)的地球化学行为在很大程度上受到其在天然辉绿锰酸盐上吸附的影响,这些辉绿锰酸盐既含有层边缘位点,也含有空位;然而,这些位点上的镉同位素分馏机制尚未得到研究。在本研究中,采用批量吸附实验、扩展 X 射线吸收精细结构 (EXAFS) 光谱、表面复合建模和密度泛函理论 (DFT) 计算相结合的方法,研究了镉在六方(包含两种类型的位点)和三菱桦锰酸盐(几乎只有边缘位点)上吸附过程中的同位素分馏。轻镉同位素在固体表面优先富集,Cd2+吸附在边缘位点上引起的同位素分馏(Δ114/110Cdedge-solution = -1.54 ± 0.11‰)小于吸附在空位上引起的同位素分馏(Δ114/110Cdvacancy-solution = -0.71 ± 0.21‰),与表面覆盖率或 pH 值无关。镉 K 边 EXAFS 和 DFT 结果都表明,在层边缘位点上形成了双角共享复合物,而在空位上主要形成了三角共享复合物。这两种络合物的变形导致了固体上的负同位素分馏,而边缘位点上镉周围稍长的第一Cd-O距离和较少的最近锰原子可能是导致分馏幅度大于空位的原因。这些结果深入揭示了镉在与植物锰酸盐相互作用过程中的同位素分馏机制。
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引用次数: 0
AOP-Anchored Transcriptome Analysis Catalogue Accelerates the Discovery of Environmental Toxicants in Zebrafish AOP 附加转录组分析目录加速了斑马鱼体内环境毒物的发现
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-17 DOI: 10.1021/acs.est.4c03100
Jierong Chen, Congcong Wang, Wenqing Tu, Kun Zhang, Karl Fent, Jiayin Dai, Markus Hecker, John P. Giesy, Yanbin Zhao
Current toxicity screening approaches to evaluate the vast number of environmental chemicals that require assessment are hampered due to their significant costs, time requirements, and reliance on live animal testing. The aim of the present study was to develop an adverse outcome pathway (AOP)-anchored transcriptome analysis (AATA) catalogue to expedite the discovery of environmental toxicants. 437 AOPs from the AOPwiki (https://aopwiki.org/) and 2280 transcriptomics data sets from NCBI Gene Expression Omnibus (GEO) and EMBL-EBI ArrayExpress (AE) repositories were comprehensively reviewed and analyzed. By using the differentially expressed molecular key event (mKE) genes as connection nodes, we created a large-scale environmental substance─target gene (mKE)─predicted adverse outcomes (SGAs) network that included 78 substances, 1099 genes, and 354 adverse outcomes (AOs). To validate the reliability of the network, comprehensive literature verification was conducted. We demonstrated that 164 of the 354 AOs identified have been previously characterized in the literature. The results for 136 of these AOs were consistent with the predictions of the AATA catalogue, representing an accuracy rate of 82.9%. Besides, distinct patterns in molecular KEs and AOs among categories of substances, such as biocides and metals, were demonstrated. Some representative substances, including atrazine and copper, pose significant risks to fish at various levels of biological organization. Moreover, experimental verification of the AATA predictions was conducted, including exposures of zebrafish to perfluorooctanesulfonate, cresyl diphenyl phosphate, and lanthanum. Results demonstrated consistency with predictions of the AATA catalogue, with an accuracy rate of 92.3%. Collectively, the present findings support the AATA catalogue as an efficient and promising platform for identifying environmental toxicants to fish and thereby provide novel insights into the understanding of potential risks of environmental contaminants.
目前评估大量需要评估的环境化学物质的毒性筛选方法因成本高、时间要求长和依赖活体动物试验而受到阻碍。本研究的目的是开发一个以不良后果途径(AOP)为导向的转录组分析(AATA)目录,以加快环境毒物的发现。研究人员全面审查和分析了 AOPwiki (https://aopwiki.org/) 中的 437 个 AOP 和 NCBI Gene Expression Omnibus (GEO) 和 EMBL-EBI ArrayExpress (AE) 数据库中的 2280 个转录组数据集。通过将差异表达的分子关键事件(mKE)基因作为连接节点,我们创建了一个大规模的环境物质-靶基因(mKE)-预测不良结果(SGAs)网络,其中包括78种物质、1099个基因和354个不良结果(AOs)。为了验证该网络的可靠性,我们进行了全面的文献验证。我们证明,在已确定的 354 个 AOs 中,有 164 个已在文献中描述过。其中 136 个 AO 的结果与 AATA 目录的预测一致,准确率为 82.9%。此外,在杀菌剂和金属等物质类别中,分子 KEs 和 AOs 也呈现出不同的模式。一些具有代表性的物质,包括阿特拉津和铜,在不同的生物组织水平上都对鱼类构成重大风险。此外,还对 AATA 预测进行了实验验证,包括让斑马鱼接触全氟辛烷磺酸、甲酚二苯基磷酸酯和镧。结果显示与 AATA 目录的预测一致,准确率为 92.3%。总之,本研究结果支持将 AATA 目录作为一个高效且有前景的平台,用于识别环境中对鱼类有毒的物质,从而为了解环境污染物的潜在风险提供新的见解。
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引用次数: 0
Assessing Transition Pathways of Hydrogen Production in China with a Probabilistic Framework 用概率框架评估中国氢气生产的过渡途径
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-17 DOI: 10.1021/acs.est.4c01304
Zihan Zhen, Xunmin Ou, Yu Wang, Sheng Zhou
The transition of China’s hydrogen production system to meeting carbon neutrality is considerably uncertain. This study uses a probabilistic framework to assess the transition pathways of hydrogen production in China to meet the goal of carbon neutrality and reveals the key technology selection mechanism. Three strategies for hydrogen production transition were considered: delayed, orderly, and radical, corresponding to the green hydrogen shares between 70 and 95% in 2060. More ambitious strategies tended to result in greater uncertainty of green hydrogen production and introduce higher system costs and cost uncertainty. The different strategies showed notable differences in carbon dioxide (CO2) reduction pathways. The cumulative CO2 emissions of the delayed strategy may reach 3 times that of the radical strategy, and the CO2 reduction uncertainty of the orderly strategy may be twice that of the other strategies. Alkaline electrolyzers were predicted to dominate green hydrogen production until being surpassed by proton exchange membrane electrolyzers (PEM) after 2060. The synergy of the solar–energy storage–PEM technology combination was notable because expensive electrolyzers tended to increase utilization, thereby diluting fixed costs. Our results underscore the importance of studying the impact of uncertainty and technology selection mechanisms on transition pathways.
中国制氢系统实现碳中和的过渡具有很大的不确定性。本研究采用概率框架评估了中国制氢向碳中和目标过渡的路径,并揭示了关键技术的选择机制。研究考虑了制氢转型的三种策略:延迟、有序和激进,分别对应 2060 年 70% 至 95% 的绿色制氢份额。更雄心勃勃的战略往往会导致绿色制氢的不确定性增加,并带来更高的系统成本和成本不确定性。不同的战略在二氧化碳(CO2)减排途径方面存在显著差异。延迟战略的累计二氧化碳排放量可能达到激进战略的三倍,有序战略的二氧化碳减排不确定性可能是其他战略的两倍。据预测,碱性电解槽将主导绿色制氢,直到 2060 年后被质子交换膜电解槽(PEM)超越。太阳能-储能-PEM 技术组合的协同效应非常显著,因为昂贵的电解槽往往会提高利用率,从而摊薄固定成本。我们的研究结果强调了研究不确定性和技术选择机制对过渡途径影响的重要性。
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引用次数: 0
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